Journal
ADVANCED MATERIALS
Volume -, Issue -, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202206450
Keywords
carbon materials; graphdiyne; N doping; sp-N; 2D materials
Categories
Funding
- National Key R&D Program of China [2018YFA0703504, 2021YFB3802600]
- National Natural Science Foundation of China [51932001, 21971244, 21820102002, 21971245]
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Scientists have achieved precise synthesis of metal-free catalysts with enhanced catalytic activity in CO2 reduction by utilizing unique doping configurations in graphdiyne. The relationship between doping configurations and reaction products has been revealed.
Due to the limited reserves of metals, scientists are devoted to exploring high-performance metal-free catalysts based on carbon materials to solve environment-related issues. Doping would build up inhomogeneous charge distribution on surface, which is an efficient approach for boosting the catalytic performance. However, doping sites are difficult to control in traditional carbon materials, thus hindering their development. Taking the advantage of unique sp-C in graphdiyne (GDY), a new N doping configuration of sp-hybridized nitrogen (sp-N), bringing a Pt-comparable catalytic activity in oxygen reduction reaction is site-defined introduced. However, the reaction intermediate of this process is never captured, hindering the understanding of the mechanism and the precise synthesis of metal-free catalysts. After the four-year study, the fabrication of intermediate-like molecule is realized, and finally sp-N doped GDY via the pericyclic reaction is obtained. Compared with GDY doped with other N configurations, the designed sp-N GDY shows much higher catalytic activity in electroreduction of CO2 toward CH4 production, owing to the unique electronic structure introduced by sp-N, which is more favorable in stabilizing the intermediate. Thus, besides opening the black-box for the site-defined doping, this work reveals the relationship between doping configuration and products of CO2 reduction.
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